Pump and probe setup

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See also: time-resolved spectroscopy , ultrafast optics , saturable absorbers , semiconductor saturable absorber mirrors , optical sampling , synchronization of lasers , laser spectroscopy and other articles in the categories optical metrology , methods.

These sharing buttons are implemented in a privacy-friendly way! Sorry, we don't have an article for that keyword! Characterization of Saturable Absorbers Pump—probe measurements can be used, for example, to monitor the recovery of a saturable absorber e. Questions and Comments from Users Here you can submit questions and comments.

Share this with your friends and colleagues, e. Buyer's Guide. It is noteworthy that the lifetime, just like the strength of the observed H bonds, correlates not only with the red shift of the respective OH stretching, but also with the magnitude of their anharmonicity, indicated by the spectral shift between GSB and ESA.

To show the spectral coverage of the 32 pixel detection, Fig. The entire transient spectrum shown in Fig. For this purpose no optical alignment is needed.

Just the internal grating of the detection setup has to be rotated. A first estimation of the temporal resolution is obtained from the FROG measurements of the pump and probe pulses.

The FWHM of the convolution between both pulses is 72 fs. Although a possible resolution of 72 fs is already quite competitive, it has to be considered that pump and probe pulses were slightly optimized to perform the FROG and CEP measurements.

A better method to determine the temporal resolution of our new spectrometer is the analysis of the transient signals. This is superior to a pure optical determination by cross correlation in a nonlinear crystal as it incorporates not only the pulse durations, but also any possible broadening mechanisms in the interaction region. Furthermore it measures the instrumental response function directly at the sample position.

In addition, no restraints as continuum generation for the CEP measurements must be regarded. As shown in Fig. To fit the experimental trace dark grey solid circles, red curve for the fit we included a coherent artifact grey curve in addition to the exponentially decaying molecular response blue curve. The coherent artifact steepens the initial rise and slightly shifts the apparent time zero.

If we do not include the artifact in the fit, an even better time resolution would be concluded. The future full analysis will clarify this situation. We can, however, be sure from both the pulse convolution and the spectroscopic measurement that the new spectrometer has a temporal resolution far better than fs.

Extracting the pulse durations from the cross correlation represented by the increase of the measured signal yields time bandwidth products of 0. The setup allows to determine transmission changes with just a strength of 1. The extracted lifetimes are in good agreement with our former measurements that rendered lifetimes of 1.

The deviation of about 1 ps for the weak bond is believed to be a result of an improved fit procedure which explicitly considers the coherent artifact. The artifact is most distinctive in the signal from the OH group engaged in the weak H bond because of the smaller red shift of the ESA. On the other hand the observation in the new recording may be due to the improved signal-to-noise ratio.

The extremely high temporal resolution and excellent sensitivity of the setup should be noted. The signal-to-noise ratio of the measurements is extremely satisfactory. The probe pulses have energies on the order of nJ. To prove the repump capability of our setup, we performed pump-repump-probe measurements in a 5M HDO in H 2 O sample at a temperature of K. When we raise the temperature of the sample by 20 K a shifted spectrum is found [ 37 ].

The difference between the two spectra is shown as dotted blue line. Since the deposition of energy into one of the high lying stretching modes yields a heating of the sample after the relaxation of the high frequency modes, this difference spectrum represents the transient response at long delay times [ 37 ].

Thus, we expect a build-up of the GSB with the instrumental response function, and a subsequent relaxation to a constant signal value, which depends on the probed spectral position and can be deduced from the stationary difference spectrum. The solid lines are fits according to a simple exponential model as guide to the eye.

The symbols represent the raw data. The delay between pump and repump pulse is set to 4. At this time the pump-repump-probe curve shows an additional signal due to further heating induced by the repump pulse absorbed by the OH stretching modes. The inset shows the absorption spectrum of the sample black, note differing scaling factors and the difference spectrum obtained by heating the sample by 20 K blue dotted.

The spectral position of pump, repump and probe pulse at the OD and OH stretch band are shown as black and red arrows. The black curve in Fig. It consists of a ground state bleaching of the OD stretching vibration around zero delay time sub fs rise. The aforementioned long-term signal is due to a spectral shift of the OD stretching band caused by heating of the sample [ 37 ]. An effective signal decay of 1. The excitation of the OH oscillators is not immediately visible in the OD stretching region, but results in an additional heating of the sample with a new rise time of 0.

This manifests itself as a clearly visible additional signal in the OD stretching vibration region and can only be observed in 3-pulse experiments.

The blue curve shows the pure repump-induced effect as a difference between the 3- and 2-pulse signal transients.

The 3. This is in striking difference to the pure signals with and without repump. From earlier work we know that the pulses of our Ti:sapphire pump system are highly correlated, i. Extended 3-pulse experiments are in progress to elucidate this combined action of OD and OH induced heating of ice. The first data presented here not only show the possibility to perform three-color experiments with excellent signal-to-noise. They also demonstrate that the high spectral tunability of the setup in combination with well engineered samples facilitates the interpretation of the data.

In this way the influence of overlapping pump-probe signals on top of the pump-repump-probe signal [ 40 ] can be minimized. In summary, we have presented a detailed description of a novel setup for IR pump-repump-probe spectroscopy with few-cycle, carrier-envelope phase stable pulses. This enables investigations on a broad variety of vibrations e. Pump and repump spectral widths are controlled by grating selectors. A first estimate of the ultrafast instrumental response function as short as 60 fs has been found.

This is even shorter than the fastest vibrational dynamics like the relaxation of the OH stretching mode in ice Ih [ 17 , 19 , 41 ] and will allow the full temporal resolution of these processes. This high sensitivity allows for measurements with extremely low pump intensities, to suppress artifacts due to strong temperature jumps [ 37 ]. The shot-to-shot stability of the presented setup is exceptionally high, allowing for high quality measurements with moderate measurement time.

A typical time-resolved measurement like the one shown in Fig. The transient spectra presented in Fig. In the future we will implement and validate a procedure that uses all 32 pixels in parallel and should decrease the recording time by more than an order of magnitude. With the available pump pulses, we have shown measurements with 8. For a thin ice sample even more than half of the OH stretch absorption is bleached. This allows the ready performance of pump-repump-probe measurements with large reasonable signal strength and excellent signal-to-noise.

In combination with the extremely high time resolution, re-excitations within the short time window spanned by the lifetime of the initially excited vibrations are possible without temporal overlap of pump and repump pulses.

Thus, we can avoid artifacts caused by the temporal overlap between pump and repump pulses. Excitations to higher lying levels will not only enable us to investigate the properties of higher lying vibrational states, but might also serve as a pathway to optically induced chemical reactions like proton transfer initiated by mid-IR pulses, which has not yet been achieved. The warming up of the system and the fine adjustment of the setup on a day-to-day basis only takes around two hours.

Thus, the visible components of the NOPA output can be employed as alignment guides. The low time consumption of both daily alignments and data recording makes the setup very suitable for the investigation of biological, short-lived samples, and enables high data output under routine operation.

Finally, it is possible to tune the pump and repump pulses to the visible and UV via minor modifications of the NOPA layouts.

This will allow us to carry out UV-pump-IR-probe experiments that can for example provide important information on the mechanisms of UV induced DNA damage or photosynthesis. Graener, G. Seifert, and A. Woutersen, U. Emmerichs, and H. Zanni and R. Khalil, N. A 27 , — Nibbering and T. Kraemer, M.

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